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1.
MoO3/Al2O3介孔催化剂在柴油氧化脱硫中的应用 总被引:1,自引:0,他引:1
通过溶胶-凝胶法,以硝酸铝为铝源、蔗糖为模板剂、氨水为沉淀剂,制备了介孔 Al2O3,并以其为载体,等体积浸渍法制备了MoO3/Al2O3介孔催化剂。采用 N2吸附-脱附及X射线衍射对介孔 Al2O3和 MoO3/Al2O3催化剂进行了表征。将 MoO3/Al2O3催化剂用于柴油催化氧化脱硫,以 H2O2为氧化剂,探讨了 MoO3负载量以及 H2O2用量对其催化柴油氧化脱硫的影响。结果表明,自制的 Al2O3载体为具有介孔结构的 γ-Al2O3,其比表面积、孔容、平均孔径分别为304.3 m2/g、 0.467 cm3/g 和6.14 nm。MoO3负载量为20%(质量分数)、H2O2与柴油中硫的摩尔比为12、氧化温度为60℃时,柴油的氧化脱硫效果较佳,脱硫率为68.4%。 相似文献
2.
复合SiO2-WO3催化剂的制备、表征及氧化脱除苯并噻吩性能 总被引:1,自引:0,他引:1
采用溶胶-凝胶法制备了SiO2-WO3催化剂,并采用XRD、FT-IR、BET、TG-DTA等方法对催化剂进行表征。以苯并噻吩(BT)为模型化合物,H2O2为氧化剂,考察了催化剂的活性元素、制备方法、n(W)/n(Si)和焙烧温度对其催化氧化脱硫活性的影响。结果表明,W的引入降低了SiO2的比表面积,SiO2-WO3催化剂中W的主物相为WO3。在以W为活性组元,且n(W)/n(Si)为0.1时,500℃焙烧得到的SiO2-0.1WO3催化剂具有最好的催化脱硫活性。在模拟油20 mL、催化剂SiO2-0.1WO3用量0.04 g、n(H2O2)/n(S)为15.9、乙腈/模拟油体积比0.3、65℃反应60 min的条件下,苯并噻吩模拟油脱硫率可达99.3%。 相似文献
3.
以钛酸丁酯为钛源、十六烷基三甲基溴化铵(CTAB)为模板剂,在超声波强化作用下制备介孔TiO2,并采用XRD、FT-IR、TG-DTA、UV-Vis、TEM和EDX分析手段对所得样品进行表征,以苯并噻吩为模型化合物,考察其光催化氧化脱硫性能。结果表明,在450℃下焙烧2 h、n(TiO2)/n(CTAB)=1/0.04的条件下,可得到球形粒子状、颗粒分布均匀、紫外光吸收边为387 nm、禁带宽度为3.32 eV、晶粒粒径6.93 nm、平均孔径3.21 nm、比表面积147.134 m2/g、孔容0.259 cm3/g的锐钛矿型介孔TiO2。在催化剂用量15 mg、H2O2作为氧化剂、nS/nO=1/200、萃取剂甲醇5 mL、吸附时间40 min、20℃反应3 h的条件下,对5 mL苯并噻吩石油醚溶液的脱硫率为98.62%。 相似文献
4.
采用共沉淀-浸渍法制备了一系列不同Ce/Co物质的量比的CeO2-Co3O4载体和CuO负载量(质量分数)为7% 的CuO/CeO2-Co3O4催化剂,考察了它们在富氢气氛中对CO的优先氧化性能。采用BET、XRD、H2-TPR等对催化剂进行了表征。测试结果表明:Ce/(Co+Ce)物质的量比为0.9时,CuO/ CeO2-Co3O4催化剂活性最好。少量的Co掺杂有利于提高催化剂的比表面积和铜物种在载体上的分散,少量的Co进入了CeO2的晶格,增强了钴铈相互作用,进而提高了载体的氧化还原性能。 相似文献
5.
制备了以γ-Al2O3为载体的Ni基选择性加氢硫转移催化剂Mo-Ni/γ-Al2O3,并用于催化裂化汽油的加氢硫转移反应。对比了预硫化型和氧化型Mo-Ni/γ-Al2O3催化剂的活性和选择性,并考察了无氧焙烧温度、活性组分负载量对预硫化型Mo-Ni/γ-Al2O3催化剂加氢硫转移催化性能的影响。采用模型化合物研究了硫醇在Mo-Ni/γ-Al2O3催化下的反应,考察了烯烃和硫醇对硫转移反应的影响。结果表明,无氧焙烧温度400℃下制备得到的w(NiO)=8.2%、w(MoS2)=5.6%的预硫化型Mo-Ni/γ-Al2O3催化剂具有相对较高的加氢硫转移反应催化活性和选择性;硫醇与烯烃的反应在催化剂表面的加氢活性位上进行,硫醇先加氢脱硫,生成吸附态H2S,吸附态H2S再与吸附的烯烃反应生成大分子硫醇或硫醚,达到硫转移的目的。 相似文献
6.
分别采用超声波辐照浸渍法和普通浸渍法制备了MnO2/γ-Al2O3催化剂,运用电感耦合等离子体原子发射光谱(ICP-AES)和X射线衍射(XRD)对催化剂进行表征,在空气-异丁醛-MnO2/γ-Al2O3体系中评价其对加氢柴油的氧化脱硫催化性能,并考察了反应温度、异丁醛用量、空气流量、溶剂类型和剂/油体积比对柴油氧化脱硫反应的影响。结果表明,超声波辐照浸渍法制备的MnO2/γ-Al2O3催化剂对柴油氧化脱硫的催化性能明显优于普通浸渍法制备的催化剂。最适宜的催化柴油氧化脱硫反应的条件为:乙腈为溶剂、加氢柴油30 mL、温度35℃、异丁醛20 mmol、空气流量0.06 L/min、超声波辐照浸渍法制备的MnO2/γ-Al2O3催化剂0.08 g、剂/油体积比1/6和催化氧化时间10 min。在此条件下可将柴油硫质量分数从542μg/g 降至31μg/g,柴油脱硫率和回收率分别为94.3%和93.3%。 相似文献
7.
制备了不同Co负载量的系列Co/γ-Al2O3催化剂,采用XRD、H2-TPR和H2-TPD等方法对其进行表征,并考察Co负载量对Co/γ-Al2O3催化剂催化F-T合成反应性能的影响。结果表明,随Co负载量的增加,Co/γ-Al2O3催化剂的催化活性先增加后降低,在Co负载量25%附近达到最大。Co/γ-Al2O3催化剂上Co3O4晶粒尺寸随Co负载量增加而逐渐增大,而催化剂的还原温度变化不大,催化剂的还原度和氢吸附量则随Co负载量增加先增大后降低。Co/γ-Al2O3催化剂的催化活性与其氢吸附量呈线性关系。 相似文献
8.
在超临界 CO2(简称 scCO2)反应介质中,TS-1催化丙烯环氧化制备环氧丙烷(PO)的 H2O2转化率,PO 选择性和 H2O2利用率要高于在传统甲醇介质中的,但是仍存在 H2O2分解和 PO 选择性较低等不足。系统研究了添加 NaOH、NaHCO3、Urea 和(NH4)2CO3碱性组分对 TS-1催化丙烯环氧化制备环氧丙烷反应的影响。结果表明,TS-1催化丙烯环氧化反应体系加入各种碱性组分均可不同程度地提高 PO 选择性,但加入 NaOH 和 NaHCO3会使H2O2分解加剧,而加入 Urea 和(NH4)2CO3则能缓解 H2O2分解,其中(NH4)2CO3的效果最好;反应体系加入0.054 mmol 的(NH4)2CO3后,H2O2转化率、PO 选择性和 H2O2利用率分别达到了97.0%、 96.8%和98.2%,从而解决了该反应在 scCO2介质中存在的H2O2分解和 PO 选择性低的问题。 相似文献
9.
采用共沉淀法制备了Al2O3-ZrO2复合氧化物,并以它为载体,浸渍法制备Cu 质量分数为24%的负载型Cu 基催化剂。运用X射线衍射(XRD)、H2程序升温还原(H2-TPR)、X射线能谱(XPS)对载体和催化剂进行表征,并考察了ZrO2对Cu/Al2O3-ZrO2催化剂糠醛选择加氢活性的影响。结果表明,载体中ZrO2质量分数20%的Cu/Al2O3-ZrO2催化剂对糠醛的选择加氢活性最高。与Cu/Al2O3催化剂相比,添加ZrO2可以提高Cu/Al2O3-ZrO2催化剂加氢活性,并有效提高较高反应温度下的糠醇选择性。 相似文献
10.
Cuo/13X分子筛的制备及其在汽油深度吸附脱硫中的应用 总被引:4,自引:0,他引:4
为有效达到汽油深度脱硫的目的,以13X分子筛为载体,采用浸渍法制备了用于催化裂化汽油深度脱硫的吸附剂CuO/13X,考察了CuO/13X的制备条件和吸附脱硫条件对其脱硫效果的影响。适宜的制备条件为CuSO_4溶液浓度0.2mol/L,浸渍时间6h,干燥温度100℃,焙烧温度350℃,焙烧时间2h;适宜的吸咐条件为常温、常压吸附,剂油比1:4,吸附时间0.5h。在最优条件下,CuO/13X对4种模拟汽油中硫的脱除率均在88%以上,CuO/13X的硫容可达4.0mg/g左右。 相似文献
11.
Abstract Due to the future specifications for sulfur content in gasoline, a lot of research work has been done to develop alternative methods for desulfurization. This work presents the results for the desulfurization by oxidation/adsorption scheme over Ti3(PW12 O40)4 catalyst. The desulfurization experiment was performed with hydrogen peroxide (H2 O2) as the oxidant in the presence of Ti3(PW12 O40)4/SiO2-Al2 O3 catalyst and adsorbent prepared by the sol-gel method, by using dibenzothiphene (DBT) in petroleum ether as the model compound. The efficiency of Ti3(PW12 O40)4/SiO2-Al2 O3 catalyst and adsorbent prepared by the sol-gel method towards DBT adsorption from model compound was studied. The effects of titanium content of the adsorbent and the reaction conditions, such as the reaction temperature, the amounts of adsorbent and hydrogen peroxide (H2 O2), and the reaction time, etc., on the desulfurization efficiency and regeneration performance of the catalyst were investigated. It was found that the Ti3(PW12 O40)4/SiO2?Al2 O3 catalyst presented higher maximum desulfurization conversion than SiO2-Al2 O3 solids. In addition, it showed higher desulfurization conversion after regeneration with N,N-dimethylamide. Optimal reaction conditions were determined as: a reaction temperature of 70°C, a Ti (titanium)/H(hydrogen) molar ratio of 3, an adsorbent amount of 5 wt%, a H2 O2/S molar ratio of 3, and a reaction time of 2 hr. As a result, the total sulfur content in the petroleum ether solution of DBT could be decreased after oxidation/adsorption scheme from an initial value of 200 μg/g to a value of 2 μg/g, and the desulfurization conversion reached 99%, which is a remarkable result. Further, the said adsorbent also had quite good regenerability. 相似文献
12.
《Petroleum Science and Technology》2013,31(11):1301-1306
Abstract Mordenite modified with Al2O3 (Al2O3/mordenite) was synthesized and used for the desulfurization of FCC gasoline. The influences of operating parameters on the results were studied for the model solution composed of dibenzothiophene (DBT) and isooctane. Al2O3/mordenite exhibits higher sulfur capacity than other kinds of chemisorbents. The suitable composition of the chemisorbent is 30 wt% Al2O3 to 70 wt% mordenite. The optimal operating parameters are: temperature 160°C; velocity 3 h?1 (WHSV). Under the stated conditions, desulfurization was carried out for the FCC gasoline with sulfur content of 220.4 μg/g. The chemisorbent can maintain the sulfur content under 50 μg/g for 40 h and has good regeneration ability after desorption using benzene. 相似文献
13.
在氢氧化铝干胶挤条成型时,调节纳米炭黑的加入量和水/粉质量比,制备了孔径呈双峰分布、具有较大孔容和比表面积的γ-Al2O3载体。当炭黑加入质量分数为13%、水/粉质量比1.15时,制备的孔径呈双峰分布的γ-Al2O3载体的孔容为0.80mL/g、比表面积为309m2/g,4~10nm和10~15nm孔径分别占总孔容50.8%和35.1%(体积分数),采用该载体制备的NiMoP/γ-Al2O3催化剂的孔径呈明显的双峰分布。在反应温度370℃、氢分压10MPa、氢/油体积比700、体积空速1.5h-1的条件下,制备的NiMoP/γ-Al2O3催化剂可使减压和焦化混合蜡油的硫质量分数由25600μg/g降至2070μg/g,脱硫率为91.9%,而参比催化剂仅可使减压和焦化混合蜡油硫质量分数降至3450μg/g,脱硫率为86.5%。 相似文献
14.
Beibei Zhang Wei Jiang Xiaonan Fan Ming Zhang Yanchen Wei Jing He Changfeng Li Huaming Li Wenshuai Zhu 《石油科学(英文版)》2018,15(4):890-897
Three amphiphilic peroxophosphomolybdates [C4mim]3PMo4O24, [C8mim]3PMo4O24 and [C16mim]3PMo4O24 were synthesized and characterized. These catalysts were used for extraction and catalytic oxidative desulfurization of fuel with H2O2 as an oxidant and ionic liquid [C4mim]BF4 as an extractant. It was found that [C16mim]3PMo4O24 showed the highest catalytic activity and the sulfur content could decrease to 7.5 ppm. In contrast, the desulfurization system shows very low performance without H2O2 or ionic liquid. The detailed reaction conditions were optimized including reaction time, temperature, the dosage of H2O2 and catalyst, and different sulfur compounds. After the reaction, the catalysts and the ionic liquid can be cycled 8 times with a little decrease in desulfurization efficiency. 相似文献
15.
A desulfurization experiment was performed with tert-butyl hydroperoxide (t-BuOOH) as the oxidant in the presence of H3PW12O40/SiO2−Al2O3 as the catalyst prepared by the sol-gel method, by using dibenzothiphene (DBT) in petroleum ether as the model compound.
This work presents the results for the desulfurization by an oxidation/catalysis/adsorption scheme. The effects of catalyst
amounts, t-BuOOH amounts, reaction temperature, and reaction time on the desulfurization efficiency and regeneration performance
of the catalyst were studied. It was found that the H3PW12O40/SiO2-Al2O3 catalyst presented a higher maximum desulfurization conversion than SiO2-Al2O3 solids also prepared by the sol-gel method. In addition, the H3PW12O40/SiO2-Al2O3 catalyst showed a higher desulfurization conversion after regeneration with N,N-dimethylamide. It was also found that the oxidation agent t-BuOOH resulted in a higher desulfurization conversion than hydrogen
peroxide (H2O2).
The text was submitted by the authors in English. 相似文献
16.
以MCM-48为载体,通过浸渍法制备了H6P2W18O62/MCM-48催化剂,并采用FT-IR、XRD、SEM、EDS对催化剂进行表征。以微波促进30%(质量分数)H2O2氧化环己酮合成己二酸反应为探针,考察了H6P2W18O62/MCM-48的催化性能,并通过正交实验确定了优化的工艺条件。结果表明,采用H6P2W18O62负载量40%的H6P2W18O62/MCM-48催化剂,在优化的合成己二酸的工艺条件下,即催化剂质量分数(以环己酮质量计)5.1%、n(C6H10O)∶n(H2O2)∶n(H2C2O4.2H2O)=100∶450∶1.88、反应温度95℃、微波功率300 W、反应时间3.5h,己二酸收率可达81.3%;催化剂重复使用5次,己二酸收率仍可达到64.6%。 相似文献
17.
A simple extraction and catalytic oxidative desulfurization (ECODS) system composed of VO(acac)2, 30% H2O2, and 1-butyl-3-methylimidazolium tetrafluoroborate ([Bmim]BF4) has been found to be suitable for the deep removal of dibenzothiophene (DBT) in model oil at room temperature. The optimal conditions were as follows: [n(H2O2)/n(DBT)/n(catalyst) = 100:20:1], model oil = 5 mL, ionic liquid [IL] = 1 mL, T = 30°C, t = 2 hr. With the ECODS system, the sulfur removal of DBT could reach 99.6%, which was superior to that of the simple extraction with IL (15.6%) or oxidation without catalyst (17.1%). The IL could be recycled five times without a significant decrease in activity. 相似文献